Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy Polymers

Abstract Sensitized triplet–triplet annihilation photon upconversion (sTTA‐UC) allows blue‐shifting non‐coherent low‐intensity light and is potentially useful in solar‐powered devices, bioimaging, 3D printing, and other applications. For technologically viable solar energy harvesting systems, solid...

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Main Authors: Xueqian Hu, Luca Pollice, Alessandra Ronchi, Marco Roccanova, Michele Mauri, Davide Lardani, Dimitri Vanhecke, Angelo Monguzzi, Christoph Weder
Format: Article
Language:English
Published: Wiley 2025-04-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202415160
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author Xueqian Hu
Luca Pollice
Alessandra Ronchi
Marco Roccanova
Michele Mauri
Davide Lardani
Dimitri Vanhecke
Angelo Monguzzi
Christoph Weder
author_facet Xueqian Hu
Luca Pollice
Alessandra Ronchi
Marco Roccanova
Michele Mauri
Davide Lardani
Dimitri Vanhecke
Angelo Monguzzi
Christoph Weder
author_sort Xueqian Hu
collection DOAJ
description Abstract Sensitized triplet–triplet annihilation photon upconversion (sTTA‐UC) allows blue‐shifting non‐coherent low‐intensity light and is potentially useful in solar‐powered devices, bioimaging, 3D printing, and other applications. For technologically viable solar energy harvesting systems, solid materials that capture a large fraction of the solar spectrum and efficiently upconvert the absorbed energy must be developed. Here, it is shown that broadband‐to‐blue UC is possible in air‐tolerant, easy‐to‐access, nanostructured polymers comprising a rigid hydrophilic matrix and liquid nanodroplets with dimensions on the order of tens of nanometers. The droplets contain 9,10‐bis[(triisopropylsilyl)ethynyl] anthracene (TIPS‐Ac) as emitter/annihilator and palladium(II) octaethyl porphyrin (PdOEP) and palladium(II) meso‐tetraphenyl tetrabenzoporphine (PdTPBP) as sensitizers. The confinement of the three dyes in the liquid domains renders the various bimolecular energy transfer processes that are pivotal for the TIPS‐Ac's triplet sensitization highly efficient, and the simultaneous use of multiple light harvesters with triplet energy levels resonant with the emitter/annihilator increases the absorption bandwidth to ca. 150 nm. The UC process at low power densities is most efficient when both sensitizers are simultaneously excited, thanks to their confinement in the nanodroplets, which leads to an increase in the triplet density, and therefore TTA rate and yield, optimizing the use of the harvested energy.
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spelling doaj-art-8f3dd931a5b74536b201d68ca2841a382025-08-20T03:09:08ZengWileyAdvanced Science2198-38442025-04-011214n/an/a10.1002/advs.202415160Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy PolymersXueqian Hu0Luca Pollice1Alessandra Ronchi2Marco Roccanova3Michele Mauri4Davide Lardani5Dimitri Vanhecke6Angelo Monguzzi7Christoph Weder8Adolphe Merkle Institute University of Fribourg Chemin des Verdiers 4 Fribourg 1700 SwitzerlandDipartimento di Scienza dei Materiali Università degli Studi Milano‐Bicocca Via Roberto Cozzi 55 Milano 20125 ItalyDipartimento di Scienza dei Materiali Università degli Studi Milano‐Bicocca Via Roberto Cozzi 55 Milano 20125 ItalyDipartimento di Scienza dei Materiali Università degli Studi Milano‐Bicocca Via Roberto Cozzi 55 Milano 20125 ItalyDipartimento di Scienza dei Materiali Università degli Studi Milano‐Bicocca Via Roberto Cozzi 55 Milano 20125 ItalyAdolphe Merkle Institute University of Fribourg Chemin des Verdiers 4 Fribourg 1700 SwitzerlandAdolphe Merkle Institute University of Fribourg Chemin des Verdiers 4 Fribourg 1700 SwitzerlandDipartimento di Scienza dei Materiali Università degli Studi Milano‐Bicocca Via Roberto Cozzi 55 Milano 20125 ItalyAdolphe Merkle Institute University of Fribourg Chemin des Verdiers 4 Fribourg 1700 SwitzerlandAbstract Sensitized triplet–triplet annihilation photon upconversion (sTTA‐UC) allows blue‐shifting non‐coherent low‐intensity light and is potentially useful in solar‐powered devices, bioimaging, 3D printing, and other applications. For technologically viable solar energy harvesting systems, solid materials that capture a large fraction of the solar spectrum and efficiently upconvert the absorbed energy must be developed. Here, it is shown that broadband‐to‐blue UC is possible in air‐tolerant, easy‐to‐access, nanostructured polymers comprising a rigid hydrophilic matrix and liquid nanodroplets with dimensions on the order of tens of nanometers. The droplets contain 9,10‐bis[(triisopropylsilyl)ethynyl] anthracene (TIPS‐Ac) as emitter/annihilator and palladium(II) octaethyl porphyrin (PdOEP) and palladium(II) meso‐tetraphenyl tetrabenzoporphine (PdTPBP) as sensitizers. The confinement of the three dyes in the liquid domains renders the various bimolecular energy transfer processes that are pivotal for the TIPS‐Ac's triplet sensitization highly efficient, and the simultaneous use of multiple light harvesters with triplet energy levels resonant with the emitter/annihilator increases the absorption bandwidth to ca. 150 nm. The UC process at low power densities is most efficient when both sensitizers are simultaneously excited, thanks to their confinement in the nanodroplets, which leads to an increase in the triplet density, and therefore TTA rate and yield, optimizing the use of the harvested energy.https://doi.org/10.1002/advs.202415160nanomaterialspolymerssolar harvestingtriplet‐triplet annihilationupconversion
spellingShingle Xueqian Hu
Luca Pollice
Alessandra Ronchi
Marco Roccanova
Michele Mauri
Davide Lardani
Dimitri Vanhecke
Angelo Monguzzi
Christoph Weder
Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy Polymers
Advanced Science
nanomaterials
polymers
solar harvesting
triplet‐triplet annihilation
upconversion
title Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy Polymers
title_full Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy Polymers
title_fullStr Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy Polymers
title_full_unstemmed Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy Polymers
title_short Confinement‐Enhanced Multi‐Wavelength Photon Upconversion Based on Triplet–Triplet Annihilation in Nanostructured Glassy Polymers
title_sort confinement enhanced multi wavelength photon upconversion based on triplet triplet annihilation in nanostructured glassy polymers
topic nanomaterials
polymers
solar harvesting
triplet‐triplet annihilation
upconversion
url https://doi.org/10.1002/advs.202415160
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